Selective reductive conversion of CO2 to CH2-bridged compounds by using a Fe-functionalized graphene oxide-based catalyst

Abstract

Anthropogenic climate change drastically affects our planet, with CO2 being the most critical gaseous driver. Despite the existing carbon dioxide capture and transformation, there is much need for innovative carbon dioxide hydrogenation catalysts with excellent selectivity. Here, we present a fast, effective, and sustainable route for coupling diverse alcohols, amines and amides with CO2 via heterogenization of a natural metal-based homogeneous catalyst through decorating on functionalized graphene oxide (GO). Combined synthetic, experimental, and theoretical studies unravel mechanistic routes to convergent 4‑electron reduction of CO2 under mild conditions. We successfully replace the toxic and expensive ruthenium species with inexpensive, ubiquitously available and recyclable iron. This iron-based functionalized graphene oxide (denoted as Fe@GO-EDA, where EDA represents ethylenediamine) functions as an efficient catalyst for the selective conversion of CO2 into a formaldehyde oxidation level, thus opening the door for interesting molecular structures using CO2 as a C1 source. Overall, this work describes an intriguing heterogeneous platform for the selective synthesis of valuable methylene-bridged compounds via 4‑electron reduction of CO2. Carbon dioxide in the atmosphere can be captured and transformed to useful chemicals with hydrogenation catalysts. Here, iron-functionalized graphene oxide-based catalyst functions as an effective catalyst for the selective conversion of carbon dioxide into a formaldehyde oxidation level.